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arXiv:quant-ph/0005118 · Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Interference at quantum transitions: lasing without inversion and resonant four-wave mixing in strong fields at Doppler-broadened transitions

Alexander K. Popov

Published Oct 21, 1998• 7 citations
arXivHTMLPDF

Abstract

An influence of nonlinear interference processes at quantum transitions in strong resonance electromagnetic fields on absorption, amplification and refractive indices as well as on four-wave mixing processes is investigated. Doppler broadening of the coupled transitions, incoherent excitation, relaxation processes, as well as power saturation processes associated with the coupled levels are taken into account. Both closed (ground state is involved) and open (only excited states are involved) energy level configurations are considered. Common expressions are obtained which allow to analyze the optical characteristics (including gain without inversion and enhanced refractive index at vanishing absorption) for various V, (Lambda) and H configurations of interfering transitions by a simple substitution of parameters. Similar expressions for resonant four-wave mixing (FWM) in Raman configurations are derived too. Crucial role of Doppler broadening is shown. Theory is applied for numerical analysis of some recent and potential experiments.

DOI
10.1117/12.328240

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Acta Physica Sinica•Jan 1, 2020•1 citation
An influence of nonlinear interference processes at quantum transitions in strong resonance electromagnetic fields on absorption, amplification and refractive indices as well as on four-wave mixing processes is investigated. Doppler broadening of the coupled transitions, incoherent excitation, relaxation processes, as well as power saturation processes associated with the coupled levels are taken into account. Both closed (ground state is involved) and open (only excited states are involved) energy level configurations are considered. Common expressions are obtained which allow to analyze the optical characteristics (including gain without inversion and enhanced refractive index at vanishing absorption) for various V, (Lambda) and H configurations of interfering transitions by a simple substitution of parameters. Similar expressions for resonant four-wave mixing (FWM) in Raman configurations are derived too. Crucial role of Doppler broadening is shown. Theory is applied for numerical analysis of some recent and potential experiments.
We study the effect of nonlinear interference processes on quantum transitions in intense resonant electromagnetic fields with allowance for changes in level populations, relaxation processes, incoherent excitation, and Doppler broadening of the transitions, on the absorption, amplification, and refraction of the interacting fields. The theory is generalized to the case of nonlinear interference interaction of two intense fields in open and closed three-level quantum systems. Using the density matrix, we derive general expressions in the case of stationary interaction that make it possible to analyze the optical characteristics for various configurations of the interfering transitions by a simple substitution of parameters. The possibility of amplifying light without saturated population inversion in a resonant transition is discussed. We formulate the conditions for such amplification and use examples to show that under appropriate changes in the initial level populations and the intensity of the auxiliary light, the inversionless amplification coefficient does not decrease with increasing intensity of the amplified radiation. We also show that allowance for these accompanying processes greatly affects the choice of optimal conditions for interference in optical transitions. As an illustration we list the results of a numerical analysis of possible experiments.
The influence of nonlinear interference processes and of changes in populations in strong electromagnetic fields, and also of the Doppler broadening on resonant four-wave frequency mixing is investigated for a system of Raman-type transitions. The case in which a quantum system interacts with one weak field and two strong fields is considered. Each of the energy levels is assumed to be perturbed by just one strong field. It is shown that the Doppler broadening alters drastically the contributions of the populations of the various levels to the investigated process and that this can alter by several orders of magnitude and nonlinear susceptibilities averaged over the velocities and influence significantly the selection of optimal configurations of the transitions and of the experimental conditions for effective resonant four-wave conversion of the radiation frequencies. A numerical analysis of the derived expressions is used to account for the experimentally observed considerable differences between the spectral dependences of the output power and the conclusions drawn from perturbation theory.
An investigation is reported of resonant four-wave frequency mixing of the type ω 4 =ω 1 —ω 2 +ω 3 under coherent population trapping conditions. Such mixing may appear when radiations of frequencies ω 1,2 are strong and when ω 1 —ω 2 =ω 20 (ω 20 is the frequency of a dipole-forbidden transition). The density matrix method is used to calculate (taking quantum interference into account) the absorption coefficients, the refractive indices, and the nonlinear susceptibilities exactly for the strong fields and in the first order of perturbation theory for the weak fields. A study is made of the dependence of the power of nonlinear optical generation on various characteristics of the transitions and of the radiation, subject to the propagation effects. The cases of homogeneous and Doppler broadening of the resonant transitions are considered. The characteristics of transitions in the barium atom are used in numerical illustrations. It is shown that the efficiency of resonant nonlinear-optical conversion of radiation can be enhanced by utilising interference processes in quantum transitions, which represent coherent population trapping.
Summary form only given.We provide additional insight into the process of resonant four-wave mixing via an analysis in the dressed states basis. As opposed to the common situation in lasing without inversion, both the excited and the ground state of the transition with enhanced coherent field generation are coupled to each other via external driving fields. For this reason we find more similarities to the well-understood process of light amplification in driven two-level systems. Initial gain does not need to arise from a spontaneous photon or a probe field but arises due to the coherence established directly by the strong external driving laser fields.
The physics of the degenerate four-wave mixing process for resonant transitions between two degenerate energy levels is investigated by direct numerical integration of the time-dependent density matrix equations. The Zeeman structure of the upper and lower energy levels is included in a multistate formulation of the density matrix equations. The inclusion of the Zeeman structure enables the investigation of the degenerate four-wave mixing process for different polarization configurations of the forward pump, backward pump, and probe beams. Saturation curves and lineshapes are calculated for different polarization configurations and for numerous low-J transitions. At low laser intensity, the results of our calculations are in excellent agreement with perturbation theory in terms of the relative intensities of the degenerate four-wave mixing signal for linear polarization configurations. As the laser intensity increases and the resonance starts to saturate, we find in general that the relative degenerate four-wave mixing reflectivity increases for the crossed polarization configurations compared to the parallel polarization configuration because the saturation intensity is higher. However, for some resonance transitions, some of the crossed polarization configurations saturate at lower laser intensities than the parallel polarization configuration, even though the reflectivity for these crossed polarization configurations is much lower than for the parallel polarization configuration in the perturbative intensity limit. This result is explained in terms of the coupling of the various Zeeman states during the degenerate four-wave mixing interaction for specific polarization configurations. The effect of saturation on the resonance line shapes for the different polarization configurations is also investigated. Finally, a limited number of calculations are performed for resonances that are Doppler broadened as well as collision broadened. The effect of saturation on the reflectivity of the crossed polarization configurations compared to the parallel polarization configuration is even more significant for resonances with comparable Doppler and collisional broadening.
We observe experimentally huge enhanced four-wave mixing based on Raman resonance in an 85Rb atomic vapor system. With the decrease of coupling field power or the increase of experimental temperature, the signal tends to be narrowed down in linewidth, and be basically the same spectrum as the stimulated Raman spectroscopy. It is found that the macroscopic polarization interference effect plays a crucial role in determining the nonlinear spectra. Further more, in the Doppler-broadened Λ-type energy level system, there is a strong relationship among electromagnetically induced transparency, four-wave mixing and stimulated Raman spectroscopy. The sharp transparent window in electromagnetically induced transparency can be interpreted as the suppression of Raman gain on the linear absorption of the probe field. However, the four-wave mixing signal is a new field generated by the atomic vapor system, and it comes from the Raman gain which is affected and modified by the absorption and dispersion of the nonlinear optical medium. It shows that in a Λ-type Doppler-broadened system, in essence, both the electromagnetically induced transparency and enhanced four-wave mixing stem from stimulated Raman scattering based on the third-order nonlinear processes, just the spectra of which are from different ways and objects of detection.